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Title: Charge-clustering induced fast ion conduction in 2LiX-GaF 3 : A strategy for electrolyte design
2LiX-GaF3(X = Cl, Br, I) electrolytes offer favorable features for solid-state batteries: mechanical pliability and high conductivities. However, understanding the origin of fast ion transport in 2LiX-GaF3has been challenging. The ionic conductivity order of 2LiCl-GaF3(3.20 mS/cm) > 2LiBr-GaF3(0.84 mS/cm) > 2LiI-GaF3(0.03 mS/cm) contradicts binary LiCl (10−12S/cm) < LiBr (10−10S/cm) < LiI (10−7S/cm). Using multinuclear7Li,71Ga,19F solid-state nuclear magnetic resonance and density functional theory simulations, we found that Ga(F,X)npolyanions boost Li+-ion transport by weakening Li+-X−interactions via charge clustering. In 2LiBr-GaF3and 2LiI-GaF3, Ga-X coordination is reduced with decreased F participation, compared to 2LiCl-GaF3. These insights will inform electrolyte design based on charge clustering, applicable to various ion conductors. This strategy could prove effective for producing highly conductive multivalent cation conductors such as Ca2+and Mg2+, as charge clustering of carboxylates in proteins is found to decrease their binding to Ca2+and Mg2+.  more » « less
Award ID(s):
1847038
PAR ID:
10490580
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
AAAS
Date Published:
Journal Name:
Science Advances
Volume:
9
Issue:
47
ISSN:
2375-2548
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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